Optically Driven Collective Spin Excitations and Magnetization Dynamics in the Néel-type Skyrmion Host GaV_{4}S_{8}.

GaV_{4}S_{8} is a multiferroic semiconductor hosting magnetic cycloid (Cyc) and Néel-type skyrmion lattice (SkL) phases with a broad region of thermal and magnetic stability. Here, we use time-resolved magneto-optical Kerr spectroscopy to show the coherent generation of collective spin excitations in the Cyc and SkL phases. Our micromagnetic simulations reveal that these are driven by an optically induced modulation of uniaxial anisotropy. Our results shed light on spin dynamics in anisotropic materials hosting skyrmions and pave a new pathway for the optical manipulation of their magnetic order.

Making Graphene Nanoribbons Photoluminescent.

We demonstrate the alignment-preserving transfer of parallel graphene nanoribbons (GNRs) onto insulating substrates. The photophysics of such samples is characterized by polarized Raman and photoluminescence (PL) spectroscopies. The Raman scattered light and the PL are polarized along the GNR axis. The Raman cross section as a function of excitation energy has distinct excitonic peaks associated with transitions between the one-dimensional parabolic subbands. We find that the PL of GNRs is intrinsically low but can be strongly enhanced by blue laser irradiation in ambient conditions or hydrogenation in ultrahigh vacuum. These functionalization routes cause the formation of sp3 defects in GNRs. We demonstrate the laser writing of luminescent patterns in GNR films for maskless lithography by the controlled generation of defects. Our findings set the stage for further exploration of the optical properties of GNRs on insulating substrates and in device geometries.

Exciton spectra and the microscopic structure of self-assembled porphyrin nanotubes.

The optical properties of tubular aggregates formed by self-assembly of zwitterionic meso-tetra(4-sulfonatophenyl)porphyrin (TPPS4) molecules are studied through a combination of experimental and theoretical techniques. The interest in these systems, with diameters of 18 nm and lengths extending up to micrometers, derives from their strong interaction with light and their similarity to natural light-harvesting systems for photosynthesis. The absorption and linear dichroism spectra are obtained in the spectral region from 300 to 750 nm, which includes the exciton bands deriving from the molecular B (Soret) as well as the Q transitions. We demonstrate that a Frenkel exciton model which takes into account the four dominant molecular excited states (Bx, By, Qx, and Qy) provides a good global fit to the experimental spectra. From comparison between theory and experiment, we propose a detailed molecular structure within the nanotube.

Resonant inelastic x-ray incarnation of Young's double-slit experiment.

Young's archetypal double-slit experiment forms the basis for modern diffraction techniques: The elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young's experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns, which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba3CeIr2O9 with structural Ir dimers and strong spin-orbit coupling. The double "slits" in this resonant experiment are the highly localized core levels of the two Ir atoms within a dimer. The clear double-slit-type sinusoidal interference patterns that we observe allow us to characterize the electronic excitations, demonstrating the power of RIXS interferometry to unravel the electronic structure of solids containing, e.g., dimers, trimers, ladders, or other superstructures.

A tunable time-resolved spontaneous Raman spectroscopy setup for probing ultrafast collective excitation and quasiparticle dynamics in quantum materials.

We present a flexible and efficient ultrafast time-resolved spontaneous Raman spectroscopy setup to study collective excitation and quasi-particle dynamics in quantum materials. The setup has a broad energy tuning range extending from the visible to near infrared spectral regions for both the pump excitation and Raman probe pulses. Additionally, the balance between energy and time-resolution can be controlled. A high light collecting efficiency is realized by high numerical aperture collection optics and a high-throughput flexible spectrometer. We demonstrate the functionality of the setup with a study of the zone-center longitudinal optical phonon and hole continuum dynamics in silicon and discuss the role of the Raman tensor in time-resolved Raman scattering. In addition, we show an evidence for unequal phonon softening rates at different high symmetry points in the Brillouin zone of silicon by means of detecting pump-induced changes in the two-phonon overtone spectrum. Demagnetization dynamics in the helimagnet Cu2OSeO3 is studied by observing softening and broadening of a magnon after photo-excitation, underlining the unique power of measuring transient dynamics in the frequency domain, and the feasibility to study phase transitions in quantum materials.

Charge and spin dynamics in a two-dimensional electron gas.

A number of time-resolved optical experiments probing and controlling the spin and charge dynamics of the high-mobility two-dimensional electron gas in a GaAs/AlGaAs heterojunction are discussed. These include time-resolved reflectivity, luminescence, transient grating, magneto-optical Kerr effect, and electro-optical Kerr effect experiments. The optical experiments provide information on the carrier lifetimes and spin dephasing times, as well as on the carrier diffusion coefficient which directly gives the charge mobility. A combination of the two types of Kerr experiment proves to be useful in extracting both the carrier lifetimes and spin dephasing times in a single experiment.

Temperature-dependent relaxation of excitons in tubular molecular aggregates: Fluorescence decay and stokes shift.

We report temperature-dependent steady-state and time-resolved fluorescence studies to probe the exciton dynamics in double-wall tubular J-aggregates formed by self-assembly of the dye 3,3'-bis(3-sulfopropyl)-5,5',6,6'-tetrachloro-1,1'-dioctylbenzimidacarbocyanine. We focus on the lowest energy fluorescence band, originating from the inner cylindrical wall. At low temperatures, the experiments reveal a nonexponential decay of the fluorescence, with a typical time scale that depends on the emission wavelength. At these temperatures we also find a dynamic Stokes shift of the fluorescence spectrum and its nonmonotonic dependence on temperature under steady-state conditions. All these data indicate that below about 20 K the excitons in the lowest fluorescence band do not reach thermal equilibrium before emission occurs, while above about 60 K thermalization on this time scale is complete. By comparing the two lowest fluorescence bands, we also find indications for fast energy transfer from the outer to the inner wall. We show that the Frenkel exciton model with diagonal disorder, which previously has been proposed to explain the absorption and linear dichroism spectra of these aggregates, yields a quantitative explanation to the observed dynamics. To this end, we extend the model to account for weak phonon-induced scattering of the localized exciton states; the spectral dynamics are then described by solving a Pauli master equation for the exciton populations.

Optically induced effective mass renormalization: the case of graphite image potential states.

Many-body interactions with the underlying bulk electrons determine the properties of confined electronic states at the surface of a metal. Using momentum resolved nonlinear photoelectron spectroscopy we show that one can tailor these many-body interactions in graphite, leading to a strong renormalization of the dispersion and linewidth of the image potential state. These observations are interpreted in terms of a basic self-energy model, and may be considered as exemplary for optically induced many-body interactions.

Dynamics of photo-excited electrons in magnetically ordered TbMnO3.

Time resolved optical spectroscopy is used to elucidate the dynamics of photodoped spin-aligned carriers in the presence of an underlying magnetic lattice in the multiferroic compound TbMnO(3). The transient responses while probing d-d intersite transitions show marked differences along different crystallographic directions, which are discussed in terms of the interplay between the processes of hopping of the photo-injected electrons and the magnetic order in the material.

Thermochromic effects in a Jahn-Teller active CuCl(4-)6 layered hybrid system.

The hybrid material copper (II) tetrachloro-bis(phenyl ethyl ammonium) (C6H5CH2CH2NH3)2CuCl4, or PEACuCl, has been investigated by temperature-dependent spectroscopic absorption experiments. The absorption bands observed in the near-infrared region (1.3-1.9 eV) generally exhibit redshifts with increasing temperature. The temperature-induced energy shifts of the spectral components are shown to be consistently related to temperature-induced Cu-Cl bond length changes. Additionally, the thermochromic color change is caused by a charge transfer band edge redshifting (in the visible region 2.0-2.8 eV) with increasing temperature. By comparison with similar Cu-based systems, it is suggested that this shift is caused by broadening and strengthening of the band.

Static magnetic susceptibility, crystal field and exchange interactions in rare earth titanate pyrochlores.

The experimental temperature dependence (T = 2-300 K) of single crystal bulk and site susceptibilities of rare earth titanate pyrochlores R(2)Ti(2)O(7) (R = Sm, Eu, Gd, Tb, Dy, Ho, Er, Yb) is analyzed in the framework of crystal field theory and a mean field approximation. Analytical expressions for the site and bulk susceptibilities of the pyrochlore lattice are derived taking into account long range dipole-dipole interactions and anisotropic exchange interactions between the nearest neighbor rare earth ions. The sets of crystal field parameters and anisotropic exchange coupling constants have been determined and their variations along the lanthanide series are discussed.

Compact cryogenic Kerr microscope for time-resolved studies of electron spin transport in microstructures.

A compact cryogenic Kerr microscope for operation in the small volume of high-field magnets is described. It is suited for measurements both in Voigt and Faraday configurations. Coupled with a pulsed laser source, the microscope is used to measure the time-resolved Kerr rotation response of semiconductor microstructures with approximately 1 mum spatial resolution. The microscope was designed to study spin transport, a critical issue in the field of spintronics. It is thus possible to generate spin polarization at a given location on a microstructure and probe it at a different location. The operation of the microscope is demonstrated by time-resolved measurements of micrometer distance diffusion of spin polarized electrons in a GaAs/AlGaAs heterojunction quantum well at 4.2 K and 7 T.

Evidence for differentiation in the iron-helicoidal chain in GdFe3(BO3)4.

A single-crystal X-ray structure study of gadolinium triiron tetraborate, GdFe3(BO3)4, at room temperature and at 90 K is reported. At room temperature GdFe3(BO3)4 crystallizes in a trigonal space group, R32 (No. 155), the same as found for other members of the iron borate family RFe3(BO3)4. At 90 K the structure of GdFe3(BO3)4 transforms to the space group P3(1)21 (No. 152). The low-temperature structure determination gives new insight into the weakly first-order structural phase transition at 156 K and into the related Raman phonon anomalies. The presence of two inequivalent iron chains in the low-temperature structure provides a new perspective on the interpretation of the low-temperature magnetic properties.

Charge-ordering signatures in the optical properties of beta-Na0.33V2O5.

Temperature dependent optical spectra are reported for beta-Na0.33V2O5. The sodium ordering transition at T(Na)=240 K and, in particular, the charge ordering transition at T(MI)=136 K strongly influence the optical spectra. The metal-insulator transition at T(MI) leads to the opening of a pseudogap ( variant Planck's over 2pi omega=1700 cm(-1)) and to the appearance of a large number of optical phonons. These observations and the presence of a midinfrared band (typical for low dimensional metals) strongly suggest that the charge carriers in beta-Na0.33V2O5 are small polarons.